This thesis examines the synthesis, photophysical properties, and sensory responses of hydroxy-substituted 1,4-distyryl-2,5-bis(arylethynyl)benzenes (Cruciforms, XFs). These two-dimensional cross-conjugated materials possess spatially separated frontier molecular orbitals (FMOs). This spatial separation allows the HOMO and LUMO to be addressed independently by analytes, which leads to significant changes in their absorption and emission. These properties allow XFs to be utilized for the detection of various analytes. These studies highlight the benefits of utilizing XFs for the development of advanced functional solid state materials for sensory applications.